Activating Lattice Oxygen in High-Entropy LDH for Robust and Durable Water Oxidation

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A high-entropy layered double hydroxide decorated with Au single atoms and oxygen vacancies exhibits low overpotential and exceptional stability for water oxidation by triggering the lattice oxygen oxidation mechanism.

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The paper studied an oxygen evolution reaction (OER) electrocatalyst, reporting a novel high-entropy MnFeCoNiCu layered double hydroxide decorated with Au single atoms and oxygen vacancies (AuSA-MnFeCoNiCu LDH) and evaluating its performance in 1.0 M KOH using electrochemical measurements alongside spectroscopic techniques and density functional theory (DFT) calculations. The authors found a low overpotential of 213 mV at 10 mA cm−2, a high mass activity of 732.925 A g−1 at 250 mV, and exceptional stability with 700 hours of continuous operation at ~100 mA cm−2. Mechanistically, they attribute improved intrinsic activity to a synergistic interaction between Au single atoms and O vacancies that upshifts the O 2p band, weakens the metal–O bond, triggers the lattice oxygen oxidation mechanism (LOM), and reduces the energy barrier. The paper explicitly presents OER performance and mechanistic evidence but, as a preprint/its provided abstract, does not state additional limitations beyond the reported experimental and modeling scope. The paper does not explicitly discuss endometriosis or adenomyosis; it was included in the corpus via a keyword match in the upstream search index.

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Abstract

Abstract The oxygen evolution reaction (OER) is known to be a kinetic bottleneck for water splitting. Triggering the lattice oxygen oxidation mechanism (LOM) can break the theoretical limit of the conventional adsorbate evolution mechanism (AEM) and enhance the OER kinetics, yet the unsatisfied stability remains a grand challenge. Here, we report a novel high-entropy MnFeCoNiCu layered double hydroxide decorated with Au single atoms and O vacancies (AuSA-MnFeCoNiCu LDH), which not only displays a low overpotential of 213 mV at 10 mA cm−2 and high mass activity of 732.925 A g−1 at 250 mV overpotential in 1.0 M KOH, but also delivers exceptional stability with 700 hours of continuous operation at ~100 mA cm−2. Combining the advanced spectroscopic techniques and density functional theory (DFT) calculations, it is demonstrated that the synergistic interaction between the incorporated Au single atoms and O vacancies leads to an upshift in the O 2p band and weakens the metal-O bond, thus triggering the LOM, reducing the energy barrier, and boosting the intrinsic activity.
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Activating Lattice Oxygen in High-Entropy LDH for Robust and Durable Water Oxidation | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Activating Lattice Oxygen in High-Entropy LDH for Robust and Durable Water Oxidation Fangqing Wang, Peichao Zou, Yangyang Zhang, Wenli Pan, Ying Li, and 4 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-2947613/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 27 Sep, 2023 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Abstract The oxygen evolution reaction (OER) is known to be a kinetic bottleneck for water splitting. Triggering the lattice oxygen oxidation mechanism (LOM) can break the theoretical limit of the conventional adsorbate evolution mechanism (AEM) and enhance the OER kinetics, yet the unsatisfied stability remains a grand challenge. Here, we report a novel high-entropy MnFeCoNiCu layered double hydroxide decorated with Au single atoms and O vacancies (AuSA-MnFeCoNiCu LDH), which not only displays a low overpotential of 213 mV at 10 mA cm −2 and high mass activity of 732.925 A g−1 at 250 mV overpotential in 1.0 M KOH, but also delivers exceptional stability with 700 hours of continuous operation at ~100 mA cm −2 . Combining the advanced spectroscopic techniques and density functional theory (DFT) calculations, it is demonstrated that the synergistic interaction between the incorporated Au single atoms and O vacancies leads to an upshift in the O 2p band and weakens the metal-O bond, thus triggering the LOM, reducing the energy barrier, and boosting the intrinsic activity. Physical sciences/Materials science/Materials for energy and catalysis/Electrocatalysis Physical sciences/Chemistry/Electrochemistry Full Text Additional Declarations There is NO Competing Interest. Supplementary Files Supportinginformation.pdf Cite Share Download PDF Status: Published Journal Publication published 27 Sep, 2023 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. 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